Phase-field based Multiscale Modeling of Heterogeneous Solid Electrolytes: Applications to Nanoporous Li 3 PS 4

Hu, Jia-Mian; Wang, Bo; Ji, Yanzhou; Yang, Tiannan; Cheng, Xiaoxing; Wang, Yi; Chen, Long-Qing

doi:10.1021/acsami.7b11292

Title: Phase-field based Multiscale Modeling of Heterogeneous Solid Electrolytes: Applications to Nanoporous Li ₃ PS ₄

Journal Article · Thu Sep 07 00:00:00 EDT 2017 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.7b11292· OSTI ID:1379179

Hu, Jia-Mian ^[1]; Wang, Bo ^[1]; Ji, Yanzhou ^[1]; Yang, Tiannan ^[1]; Cheng, Xiaoxing ^[1]; Wang, Yi ^[1]; Chen, Long-Qing ^[1]

Pennsylvania State Univ., University Park, PA (United States). Dept. of Materials Science and Engineering

Modeling the effective ion conductivities of heterogeneous solid electrolytes typically involves the use of a computer-generated microstructure consisting of randomly or uniformly oriented fillers in a matrix. But, the structural features of the filler/matrix interface, which critically determine the interface ion conductivity and the microstructure morphology, have not been considered during the microstructure generation. In using nanoporous β-Li₃PS₄ electrolyte as an example, we develop a phase-field model that enables generating nanoporous microstructures of different porosities and connectivity patterns based on the depth and the energy of the surface (pore/electrolyte interface), both of which are predicted through density functional theory (DFT) calculations. Room-temperature effective ion conductivities of the generated microstructures are then calculated numerically, using DFT-estimated surface Li-ion conductivity (3.14×10^-3 S/cm) and experimentally measured bulk Li-ion conductivity (8.93×10^-7 S/cm) of β-Li₃PS₄ as the inputs. We also use the generated microstructures to inform effective medium theories to rapidly predict the effective ion conductivity via analytical calculations. Furthemore, when porosity approaches the percolation threshold, both the numerical and analytical methods predict a significantly enhanced Li-ion conductivity (1.74×10^-4 S/cm) that is in good agreement with experimental data (1.64×10^-4 S/cm). The present phase-field based multiscale model is generally applicable to predict both the microstructure patterns and the effective properties of heterogeneous solid electrolytes.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: FG02-07ER46417; DMR-1410714; DMR-1629270

OSTI ID:: 1379179

Journal Information:: ACS Applied Materials and Interfaces, Vol. 9, Issue 38; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
solid electrolytes
ion conductivity
density functional theory
phase-field modeling
effective medium theory

Title: Phase-field based Multiscale Modeling of Heterogeneous Solid Electrolytes: Applications to Nanoporous Li 3 PS 4

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Title: Phase-field based Multiscale Modeling of Heterogeneous Solid Electrolytes: Applications to Nanoporous Li ₃ PS ₄